Abstract: | Controlled growth of high‐quality patterned perovskite films on a large scale is essentially required for the application of this class of materials in functional integrated devices and systems. Herein, graphene‐assisted hydrophilic–hydrophobic surface‐induced growth of Cs‐doped FAPbI3 perovskite films with well‐patterned shapes by a one‐step spin‐coating process is developed. Such a facile fabrication technique is compatible with a range of spin‐coated perovskite materials, perovskite manufacturing processes, and substrates. By employing this growing method, controllable perovskite photodetector arrays are realized, which have not only prominent photoresponse properties with a responsivity and specific detectivity of 4.8 AW?1 and 4.2 × 1012 Jones, respectively, but also relatively small pixel‐to‐pixel variation. Moreover, the photodetectors array can function as an effective visible light image sensor with a decent spatial resolution. Holding the above merits, the proposed technique provides a convenient and effective pathway for large‐scale preparation of patterned perovskite films for multifunctional application purposes. |